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无机、合成及天然螯合剂对铁(II)介导的氯酚类物质高级氧化的影响。

Effect of inorganic, synthetic and naturally occurring chelating agents on Fe(II) mediated advanced oxidation of chlorophenols.

作者信息

Rastogi Aditya, Al-Abed Souhail R, Dionysiou Dionysios D

机构信息

Department of Civil and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221-0071, USA.

出版信息

Water Res. 2009 Feb;43(3):684-94. doi: 10.1016/j.watres.2008.10.045. Epub 2008 Nov 6.

DOI:10.1016/j.watres.2008.10.045
PMID:19038413
Abstract

This study examines the feasibility and application of Advanced Oxidation Technologies (AOTs) for the treatment of chlorophenols that are included in US EPA priority pollutant list. A novel class of sulfate/hydroxyl radical-based homogeneous AOTs (Fe(II)/PS, Fe(II)/PMS, Fe(II)/H2O2) was successfully tested for the degradation of series of chlorophenols (4-CP, 2,4-CP, 2,4,6-CP, 2,3,4,5-CP). The major objective of the present study was to evaluate the effectiveness of three representative chelating agents (citrate, ethylenediaminedisuccinate (EDDS), and pyrophosphate) on Fe(II)-mediated activation of three common peroxide (peroxymonosulfate (PMS), persulfate (PS), and hydrogen peroxide (H2O2)) at neutral pH conditions. Short term (4 h) and long term (7 days) experiments were conducted to evaluate the kinetics and longevity of different oxidative systems for 4-chlorophenol degradation. Results showed that each of the iron-chelating agent couple was superior in activating a particular oxidant and consequently for 4-CP degradation. In case of Fe(II)/PMS system, the inorganic chelating agent pyrophosphate showed effective activation of PMS whereas very fast dissociation of PMS was recorded in the case of EDDS without any apparent 4-CP degradation. In Fe(II)/H2O2 system, EDDS was proven to be the most effective whereas pyrophosphate showed negligible activation of H2O2. Fe(II)/Citrate system showed moderate activation of all three oxidants. PMS was found to be the most universal oxidant, which was activated by all three iron-chelating agent systems and Fe(II)/Citrate was the most universal chelating agent system, which was able to activate all three oxidants to a certain extent.

摘要

本研究考察了高级氧化技术(AOTs)处理美国环保署优先污染物名单中氯酚的可行性及应用。成功测试了一类新型基于硫酸根/羟基自由基的均相AOTs(Fe(II)/过硫酸盐(PS)、Fe(II)/过一硫酸盐(PMS)、Fe(II)/过氧化氢(H2O2))对一系列氯酚(4-氯酚(4-CP)、2,4-二氯酚(2,4-CP)、2,4,6-三氯酚(2,4,6-CP)、2,3,4,5-四氯酚(2,3,4,5-CP))的降解效果。本研究的主要目的是评估三种代表性螯合剂(柠檬酸盐、乙二胺二琥珀酸(EDDS)和焦磷酸盐)在中性pH条件下对Fe(II)介导的三种常见过氧化物(过一硫酸盐(PMS)、过硫酸盐(PS)和过氧化氢(H2O2))活化的有效性。进行了短期(4小时)和长期(7天)实验,以评估不同氧化体系降解4-氯酚的动力学和持久性。结果表明,每对铁螯合剂在活化特定氧化剂以及因此降解4-CP方面都具有优势。在Fe(II)/PMS体系中,无机螯合剂焦磷酸盐显示出对PMS的有效活化,而在EDDS存在的情况下记录到PMS非常快速的分解,且没有明显的4-CP降解。在Fe(II)/H2O2体系中,EDDS被证明是最有效的,而焦磷酸盐对H2O2的活化可忽略不计。Fe(II)/柠檬酸盐体系对所有三种氧化剂均显示出适度的活化。发现PMS是最通用的氧化剂,它被所有三种铁螯合剂体系活化,并且Fe(II)/柠檬酸盐是最通用的螯合剂体系,它能够在一定程度上活化所有三种氧化剂。

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